Preparation and catalytic properties of cobalt salts of Keggin type heteropolyacids supported on mesoporous silica

被引:13
作者
Popa, Alexandru [1 ]
Sasca, Viorel [1 ]
Verdes, Orsina [1 ]
Oszko, Albert [2 ]
机构
[1] Inst Chem Timisoara, Bl Mihai Viteazul 24, Timisoara 300223, Romania
[2] Univ Szeged, Inst Phys Chem & Mat Sci, Aradi Vertanuk Tere 1, H-6720 Szeged, Hungary
关键词
Cobalt molybdophosphate; Mesoporous silica; Tween; 60; XPS analysis; Temperature programmed desorption; Ethanol conversion; GAS-SOLID INTERFACE; SELECTIVE OXIDATION; OXYGEN-TRANSFER; ACID CATALYSTS; DEHYDRATION; ETHANOL; POLYOXOMETALATE; PERFORMANCE; ALCOHOLS; CSXH3-XPW12O40;
D O I
10.1016/j.cattod.2017.02.045
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Some heteropoly salts - mesoporous silica composites were prepared from Co salt of molybdophosphoric acid CoHPMo12O40(CoHPM) by supporting on mesoporous silica in different concentrations (20-40 wt% CoHPM) of active phase. The acidity of composites was studied by the adsorption of ammonia and its temperature programmed desorption - TPD using thermogravimetry. The evolved gases during the adsorption-desorption of ammonia on CoPM-silica composites were identified by online mass spectrometry coupled with thermal gravimetry technique. The elemental concentrations based on the relative area of XPS spectra components for Co 2p, Mo 3d, Si 2p and O 1s were obtained for the surface of CoHPM/silica. The dehydration of ethanol was used to probe the catalytic properties of the CoHPM samples incorporated on the silica matrix. The main reaction products obtained on acid (dehydration) catalytic centres were ethylene and diethyl ether, besides acetaldehyde which was obtained on redox (dehydrogenation) catalytic centres. It is shown that silica - supported catalysts, appeared to be more active than bulk CoHPM catalyst in dehydration and dehydrogenation reactions. The higher values of dehydration and reaction products formation are obtained with the lowest loading (20 wt% CoHPM) and as a consequence the highest dispersion of active phase. The ethanol conversion and the carbon selectivity to the primary compounds were investigated during time on stream in order to study the stability and regenerability of supported catalysts. (c) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:233 / 242
页数:10
相关论文
共 48 条
[1]   Solid acid catalysts based on H3PW12O40 heteropoly acid Acid and catalytic properties at a gas-solid interface [J].
Alsalme, Ali M. ;
Wiper, Paul V. ;
Khimyak, Yaroslav Z. ;
Kozhevnikova, Elena F. ;
Kozhevnikov, Ivan V. .
JOURNAL OF CATALYSIS, 2010, 276 (01) :181-189
[2]   Reactivity of Heteropolytungstate and Heteropolymolybdate Metal Transition Salts in the Synthesis of Dimethyl Carbonate from Methanol and CO2 [J].
Aouissi, Ahmed ;
Al-Deyab, Salem S. ;
Al-Owais, Ahmad ;
Al-Amro, Amro .
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES, 2010, 11 (07) :2770-2779
[3]   Preparation and characterization of HMS supported 11-molybdo-vanado-phosphoric acid for selective oxidation of propylene [J].
Benadji, S. ;
Eloy, P. ;
Leonard, A. ;
Su, B. L. ;
Bachari, K. ;
Rabia, C. ;
Gaigneaux, E. M. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2010, 130 (1-3) :103-114
[4]   Characterization of H3+xPMo12-xVxO40 heteropolyacids supported on HMS mesoporous molecular sieve and their catalytic performance in propene oxidation [J].
Benadji, Siham ;
Eloy, Pierre ;
Leonard, Alexandre ;
Su, Bao-Lian ;
Rabia, Cherifa ;
Gaigneaux, Eric M. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2012, 154 :153-163
[5]   Heteropolyacid supported on montmorillonite catalyst for dehydration of dilute bio-ethanol [J].
Bokade, Vijay V. ;
Yadav, Ganapati D. .
APPLIED CLAY SCIENCE, 2011, 53 (02) :263-271
[6]   Compensation effect in isopropanol dehydration over heteropoly acid catalysts at a gas-solid interface [J].
Bond, Geoffrey C. ;
Frodsham, Sarah J. ;
Jubb, Paul ;
Kozhevnikova, Elena F. ;
Kozhevnikov, Ivan V. .
JOURNAL OF CATALYSIS, 2012, 293 :158-164
[7]   An efficient, catalytic, aerobic, oxidative iodination of arenes using the H5PV2Mo10O40 polyoxometalate as catalyst [J].
Branytska, OV ;
Neumann, R .
JOURNAL OF ORGANIC CHEMISTRY, 2003, 68 (24) :9510-9512
[8]  
Carretero M, 2012, INT REV HIST EDUC, P1
[9]   XPS study of as-prepared and reduced molybdenum oxides [J].
Choi, JG ;
Thompson, LT .
APPLIED SURFACE SCIENCE, 1996, 93 (02) :143-149
[10]   Redox behavior and oxidation catalysis of HnXW12O40 (X = Co2+, B3+, Si4+, and P5+) Keggin heteropolyacid catalysts [J].
Choi, Jung Ho ;
Kang, Tae Hun ;
Song, Ji Hwan ;
Bang, Yongju ;
Song, In Kyu .
CATALYSIS COMMUNICATIONS, 2014, 43 :155-158